Efficient catalysts of surface hydrophobic Cu-BTC with coordinatively unsaturated Cu(I) sites for the direct oxidation of methane.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 36848552.
- Also identified by DOI 10.1073/pnas.2206619120 and PMC identifier 10013780.
- Licence recorded as CC BY-NC-ND.
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Abstract
Selective oxidation of methane to organic oxygenates over metal-organic frameworks (MOFs) catalysts at low temperature is a challenging topic in the field of C1 chemistry because of the inferior stability of MOFs. Modifying the surface of Cu-BTC via hydrophobic polydimethylsiloxane (PDMS) at 235 °C under vacuum not only can dramatically improve its catalytic cycle stability in a liquid phase but also generate coordinatively unsaturated Cu(I) sites, which significantly enhances the catalytic activity of Cu-BTC catalyst. The results of spectroscopy characterizations and theoretical calculation proved that the coordinatively unsaturated Cu(I) sites made H<sub>2</sub>O<sub>2</sub> dissociative into •OH, which formed Cu(II)-O active species by combining with coordinatively unsaturated Cu(I) sites for activating the C-H bond of methane. The high productivity of C1 oxygenates (CH<sub>3</sub>OH and CH<sub>3</sub>OOH) of 10.67 mmol g<sub>cat.</sub><sup>-1</sup>h<sup>-1</sup> with super high selectivity of 99.6% to C1 oxygenates was achieved over Cu-BTC-P-235 catalyst, and the catalyst possessed excellent reusability.